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Enhanced Performance of Ceria-Based NO_x Reduction Catalysts by Optimal Support Effect

机译:最佳支持效应增强二氧化铈基NO_x还原催化剂的性能

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摘要

CeO_2-based catalysts have attracted widespread attention in environmental-protection applications; including selective catalytic reduction (SCR) of NO by NH_3, and their catalytic performance is often intimately associated with the supports used. However, the issue of how to choose the supports of such catalysts still remains unresolved. Herein, we systematically study the support effect in SCR over CeO_2-based catalysts by using three representative supports, Al_2O_3, TiO_2, and hexagonal WO_3 (HWO), with different acidic and redox properties. HWO, with both acidic and reducible properties, achieves an optimal support effect; that is, CeO_2/HWO exhibits higher catalytic activity than CeO_2 supported on acidic AI_2O_3 or reducible TiO_2. Transmission electron microscopy and X-ray diffraction techniques demonstrate that acidic supports (HWO and Al_3O_3) are fevorable for the dispersion of CeO_2 on their surfaces. X-ray photoelectron spectroscopy coupled with theoretical calculations reveals that reducible supports (HWO and TiO_2) facilitate strong electronic Ce_2-support interactions. Hence, the excellent catalytic performance of CeO_2/HW0 is mainly ascribed to the high dispersion of CeO_2 and the optimal electronic CeO_2-support interactions. This work shows that abundant Brønsted acid sites and excellent redox ability of supports are two criticd requirements for the design of efficient CeO_2-based catalysts.
机译:基于CeO_2的催化剂在环境保护应用中已引起广泛关注;包括NH_3选择性催化还原NO(SCR),其催化性能通常与所用载体密切相关。但是,如何选择这种催化剂的载体的问题仍然没有解决。在本文中,我们通过使用具有不同酸性和氧化还原特性的三种代表性载体Al_2O_3,TiO_2和六方WO_3(HWO),系统地研究了SCR对CeO_2基催化剂的催化作用。具有酸性和可还原性质的HWO达到最佳的载体作用;即CeO_2 / HWO的催化活性高于酸性AI_2O_3或可还原TiO_2上负载的CeO_2。透射电子显微镜和X射线衍射技术表明,酸性载体(HWO和Al_3O_3)有利于CeO_2在其表面上的分散。 X射线光电子能谱结合理论计算表明,可还原的载体(HWO和TiO_2)促进了强的Ce_2-电子电子相互作用。因此,CeO_2 / HW0的优异催化性能主要归因于CeO_2的高分散性和最佳的电子CeO_2-载体相互作用。这项工作表明,丰富的布朗斯台德酸位点和出色的载体氧化还原能力是设计高效CeO_2基催化剂的两个受到批评的要求。

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  • 来源
    《Environmental Science & Technology》 |2017年第1期|473-478|共6页
  • 作者单位

    Institute of Atmospheric Sciences, Shanghai Key Laboratory of Atmospheric Particle Pollution & Prevention, Department of Environmental Science & Engineering, Fudan University, Shanghai 200433, China;

    Institute of Atmospheric Sciences, Shanghai Key Laboratory of Atmospheric Particle Pollution & Prevention, Department of Environmental Science & Engineering, Fudan University, Shanghai 200433, China;

    Institute of Atmospheric Sciences, Shanghai Key Laboratory of Atmospheric Particle Pollution & Prevention, Department of Environmental Science & Engineering, Fudan University, Shanghai 200433, China;

    Institute of Atmospheric Sciences, Shanghai Key Laboratory of Atmospheric Particle Pollution & Prevention, Department of Environmental Science & Engineering, Fudan University, Shanghai 200433, China;

    Institute of Atmospheric Sciences, Shanghai Key Laboratory of Atmospheric Particle Pollution & Prevention, Department of Environmental Science & Engineering, Fudan University, Shanghai 200433, China;

    Institute of Atmospheric Sciences, Shanghai Key Laboratory of Atmospheric Particle Pollution & Prevention, Department of Environmental Science & Engineering, Fudan University, Shanghai 200433, China;

    Institute of Atmospheric Sciences, Shanghai Key Laboratory of Atmospheric Particle Pollution & Prevention, Department of Environmental Science & Engineering, Fudan University, Shanghai 200433, China,Jiangsu Collaborative Innovation Center of Atmospheric Environment and Equipment Technology, Nanjing University of Information Science & Technology, Nanjing 210044, China;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
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  • 正文语种 eng
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